Year of publication:
Journal of Vacuum Science & Technology A
One of the many contributions of Harold Winters to
surface science was his pioneering ultrahigh vacuum study on the kinetics of the technologically important dissociation of CH4 on transition metals in the 1970s. He observed a dramatic activation of the dissociation with surface temperature alone and a huge isotope effect and suggested a simple dynamical model to rationalize his results. Since that time, our general understanding of the dynamics of gas-surface dissociations has exploded due to experimental advances (e.g., molecular beam and eigenstate resolved studies) and theoretical advances (quantum or classical dynamics on ab initio potential energy surfaces). This review tries to highlight how our understanding of the dynamics of CH4 dissociation on transition metals has matured since Harold's pioneering experiments and original model.